The single-Mo-atom-embedded-graphdiyne monolayer with ultra-low onset potential as high efficient electrocatalyst for N2 reduction reaction
The single-Mo-atom-embedded-graphdiyne monolayer with ultra-low onset potential as high efficient electrocatalyst for N2 reduction reaction
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具有超低起始电位的单Mo原子嵌入石墨二炔单层作为N2还原反应的高效电催化剂
DOI：
10.1016/j.apsusc.2019.144941
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发表时间：
2020-03
影响因子：
6.7
通讯作者：
Jinli Zhang
中科院分区：
文献类型：
--
作者：
Xingwu Zhai;Hongxia Yan;Guixian Ge;Jueming Yang;Feng Chen;Xiaoyue Liu;Dezheng Yang;Linfeng Li;Jinli Zhang
在化学工业中，在环境条件下生产氨（NH3）一直面临着巨大的挑战。本文采用密度泛函理论（DFT）方法，系统地研究了过渡金属（TM = Sc，Cr，Mn，Fe，Co，Ni，Cu，Zn，Mo，Ru，Rh，Pd和Ag）嵌入石墨二炔单分子膜（TM@GDY）电催化剂在N2还原反应（NRR）中的电位.结果表明，Mo包埋石墨二炔单分子膜（Mo@GDY）具有高稳定性、高电导率和优异的催化活性，其起始电位为-0.33 V，属于远端机理。超低起始电位归因于在第一次氢化期间，与酶促机制（-1.03 V）相比，远端机制的氢与下一个最近的氮原子（H-N2）之间的相互作用强得多。此外，Mo@GDY还可以有效抑制整个NRR过程中的析氢反应（HER）。该研究为常温下电化学还原N2生成NH3提供了一种新的途径。
The production of ammonia (NH3) at ambient conditions has always faced enormous challenges in chemical industry. In this study, the potential of the electrocatalysts of transition-metal-embedded (TM = Sc, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Ru, Rh, Pd and Ag) graphdiyne monolayer (TM@GDY) has been systematically investigated as nitrogen (N2) Reduction Reaction (NRR) by Density Functional Theory (DFT). The results reveal that Mo-embedded graphdiyne monolayer (Mo@GDY) has high stability, high electrical conductivity and excellent catalytic activity with ultra-low onset potential (−0.33 V) by distal mechanism. The ultra-low onset potential is attributed to much stronger interactions between hydrogen and the next nearest nitrogen atoms (H-N2) for the distal mechanism compared with the enzymatic mechanism (−1.03 V) during the first hydrogenation. Moreover, Mo@GDY can also effectively suppress the Hydrogen Evolution Reaction (HER) during the entire NRR process. This study may provide a new approach for electrochemical N2reduction to form NH3at ambient conditions.
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DOI：
10.1002/recl.19270460805
发表时间：
2010-09
期刊：
Recueil des Travaux Chimiques des Pays-Bas
影响因子：
--
作者：
J. Heyrovský
通讯作者：
J. Heyrovský
影响因子：
64.8
作者：
van Kessel MA;Speth DR;Albertsen M;Nielsen PH;Op den Camp HJ;Kartal B;Jetten MS;Lücker S
通讯作者：
Lücker S
影响因子：
15
作者：
Jingxiang Zhao;Zhongfang Chen
通讯作者：
Jingxiang Zhao;Zhongfang Chen
DOI：
10.1126/science.1224603
发表时间：
2012-09-28
期刊：
Science (New York, N.Y.)
影响因子：
--
作者：
Wiig JA;Hu Y;Chung Lee C;Ribbe MW
通讯作者：
Ribbe MW
影响因子：
16.6
作者：
Kitano, Masaaki;Kanbara, Shinji;Inoue, Yasunori;Kuganathan, Navaratnarajah;Sushko, Peter V.;Yokoyama, Toshiharu;Hara, Michikazu;Hosono, Hideo
通讯作者：
Hosono, Hideo